全部 标题 作者
关键词 摘要

OALib Journal期刊
ISSN: 2333-9721
费用:99美元

查看量下载量

相关文章

更多...

醋酸溶液中pd-cupc/y催化甲烷选择氧化制甲醇

, PP. 985-990

Keywords: 酞菁,,分子筛,甲烷,甲醇,醋酸

Full-Text   Cite this paper   Add to My Lib

Abstract:

?以氯化铜、钼酸铵、苯酐、氯化铵、尿素和nay分子筛为原料,采用苯酐-尿素法制备了酞菁铜/分子筛复合物cupc/y.采用等体积浸渍法将金属钯担载在cupc/y上制备了pd-cupc/y催化剂,并在醋酸水溶液中考察了其催化甲烷选择氧化合成甲醇反应的性能,结果表明,催化性能与反应温度、溶剂中ch3cooh与h2o的混合比例、对苯醌用量、反应时间等因素有关,在0.5%pd-0.5%cupc/y添加量0.5g、ch3cooh与h2o体积比4∶1、对苯醌用量1000μmol、反应时间3h、反应温度150℃的条件下,甲醇的最佳生成量为1840μmol.pd-cupc/y催化剂可以多次循环使用,但由于催化剂流失和催化剂表面的钯粒子聚集的原因,循环使用后的催化剂催化活性有所下降.pd-cupc/y在醋酸溶液中催化甲烷选择氧化合成甲醇是亲电取代反应和活性氧物种氧化共同作用的结果.

References

[1]  陈立宇,杨伯伦,张秀成.甲烷直接液相转化合成甲醇的研究进展[j].石油化工,2002,31(11):938-942.(chenli-yu,yangbo-lun,zhangxiu-cheng.progressindirectconversionofmethanetomethanolinliquidphase[j].petrochemicaltechnology,2002,31(11):938-942.)
[2]  linmr,sena.directcatalyticconversionofmethanetoaceticacidinanaqueousmedium[j].nature,1994,368(6472):613-615.
[3]  yuanq,dengwp,zhangqh,wangy.osmium-catalyzedselectiveoxidationsofmethaneandethanewithhydrogenperoxideinaqueousmedium[j].advsynthcatal,2007,349(7):1199-1209.
[4]  perianara,taubedj,evitter,lofflerdg,wentrcekpr,vossg,masudat.amercury-catalyzed,high-yieldsystemfortheoxidationofmethanetomethanol[j].science,1993,259(5093):340-343.
[5]  shilovae,shul'pingb.activationofc-hbondsbymetalcomplexes[j].chemrev,1997,97(8):2879-2932.
[6]  michalkiewiczb,kaluckik,sosnickijg.catalyticsystemcontainingmetallicpalladiumintheprocessofmethanepartialoxidation[j].jcatal,2003,215(1):14-19.
[7]  魏新,叶林敏,祝明霞,袁友珠.发烟硫酸中pd/c催化甲烷选择氧化制甲醇[j].催化学报,2008,29(8):720-726.(weixin,yelin-min,zhuming-xia,yuanyou-zhu.selectiveoxidationofmethanetomethanolinoleumoverpd/ccatalyst[j].chinjcatal,2008,29(8):720-726.)
[8]  perianara,mirinovo,taubedj,gambles.highyieldconversionofmethanetomethylbisulfatecatalyzedbyiodinecations[j].chemcommun,2002,(20):2376-2377.
[9]  chenly,yangbl,zhangxc,dongw,zhangxp.methanepartialoxidationinliquidphaseusingvanadium-containingheteropolyacidcatalystsinoleum[j].chinjcatal,2006,27(6):462-463.
[10]  tryndal.complexesofiron,cobaltandcoppertetrasulfonatedphthalocyanineswithapomyoglobin[j].inorgchimacta,1983,78(5):229-237.
[11]  ratnasamyp,srinivasad.selectiveoxidationsoverzeoliteandmesoporoussilica-basedcatalysts:selectedexamples[j].cataltoday,2009,141(1/2):3-11.
[12]  张昕,贺德华,张启俭,朱起明.甲烷气相均相选择氧化合成甲醇[j].石油化工,2003,32(3):195-199.(zhangxin,hede-hua,zhangqi-jian,zhuqi-ming.studiesongas-phasehomogeneousselectiveoxidationofmethanetomethanol[j].petrochemicaltechnology,2003,32(3):195-199.)
[13]  樊亚芳,王春雷,马丁,包信和.室温下钯-金属酞菁/分子筛复合催化剂催化甲烷选择氧化制甲醇[j].催化学报,2010,31(3):302-306.(fanya-fang,wangchun-lei,mading,baoxin-he.selectiveoxidationofmethanetomethanoloverpalladium-metallophthalocyaninecompositecatalystsatroomtemperature[j].chinesejournalofcatalysis,2010,31(3):302-306.)
[14]  徐锋,朱丽华,侯凤才,沈斌.醋酸溶液中pd(oac)2-对苯醌-co催化甲烷选择氧化制甲醇[j].燃料化学学报,2012,40(9):1098-1102.(xufeng,zhuli-hua,houfeng-cai,shenbin.selectiveoxidationofmethanetomethanoloverpd(oac)2-p-benzoquinone-cocatalystsysteminaceticacidsolvent[j].journaloffuelchemistryandtechnology,2012,40(9):1098-1102.)
[15]  徐锋,朱丽华.甲烷液相部分氧化制甲醇的动力学影响因素[j].石油化工,2012,41(10):1137-1142.(xufeng,zhuli-hua.kineticinfluencingfactorsforpartialoxidationofmethanetomethanolinliquidphase[j].petrochemicaltechnology,2012,41(10):1137-1142.)
[16]  xuf,zhulh,biyw,houfc.researchonreactionmechanismofminegaspartialoxidationintomethanolinaceticacid[j].resjchemenviron,2012,16(s1):122-126.
[17]  metzj,schneidero,hanackm.synthesisandpropertiesofsubstituted(phthalocyaninato)-ironand-cobaltcompoundsandtheirpyridineadducts[j].inorgchem,1984,23(8):1065-1071.
[18]  夏雪伟,徐庆锋,路建美,姚社春,王丽华,陈飞,朱秀林.金属酞菁配合物的合成及其三阶非线性光学性能研究[j].高校化学工程学报,2007,2(1):131-135.(xiaxue-wei,xuqing-feng,lujian-mei,yaoshe-chun,wangli-hua,chenfei,zhuxiu-lin.third-ordernonlinearopticalpropertiesofmetalphthalocyaninecomplex:effectofcentralmetalions[j].journalofchemicalengineeringofchineseuniversities,2007,2(1):131-135.)
[19]  范彬彬,李瑞丰,樊卫斌,曹景慧,钟炳.cupc/y分子筛制备与性能的研究[j].石油学报(石油加工),2000,16(1):12-16.(fanbin-bin,lirui-feng,fanwei-bin,caojing-hui,zhongbing.studiesonpreparationandcharacteristicsofcupc/yzeolites[j].actapetroleisinica(petroleumprocessingsection),2000,16(1):12-16.)
[20]  shilovae,shulpingb.activationofc-hbondsbymetalcomplex[j].chemrev,1997,97(8):2879-2932.

Full-Text

Contact Us

service@oalib.com

QQ:3279437679

WhatsApp +8615387084133